Reactive hot-melt-type adhesive granulate for insulating glass

ABSTRACT

The invention relates to a reactive batch of thermoplastic polymer particles on the basis of poly-α-olefins, elastomeric block copolymers and/or polyisobutylenes. Said batch is useful for producing insulating glass units consisting of two or several glass panes, casting resin panes, solar collectors or facade elements for edifices. The reactive batch contains a portion of batch particles which contain polymers with reactive groups selected from hydroxyl groups, amino groups, carboxyl groups, carboxylic acid anhydride groups. mercapto groups, hydrosilicon groups and/or hydrosilyl groups. Another portion of the batch particles contains polymers with reactive groups that are complementary thereto and are selected from isocyanate groups, epoxide groups, active olefinically unsaturated double bonds and/or water-producing substances. Said batch of reactive particles is homogenised only directly before the last use and, immediately afterwards, is applied to the substrate surfaces to be connected. Dosing problems have not been observed with respect to this kind of reactive granulates.

[0001] This invention relates to a reactive blend of thermoplasticpolymer particles and to a process for the production of two-panel ormulti-panel insulating glass.

[0002] Two-panel or multi-panel insulating glass composite systemsconsist of two or more glass panels which are arranged parallel to oneanother and which are joined at their edges in such a way that the gapbetween the panels is sealed off from the ambient air so that it cannotbe penetrated by moisture. In addition, the edge seal is designed insuch a way that it is able to withstand all the mechanical and chemicalstresses caused by varying climatic conditions. In many cases, the gapbetween the panels is filled with dry gases which increase heat or soundinsulation in relation to the normal air filling. Insulating glass ofthe type in question is mainly used in the building industry, but alsoin vehicle manufacture.

[0003] The edge seal of such insulating glass can be formed in differentways. In what is still the most common version, a hollow aluminium orsteel profile acts as a spacer for the required gap between the glasspanels. It is arranged near the edges of the glass panels so that thespacer together with the edges of the glass panels forms an outwardlyfacing channel for accommodating sealants and adhesives. These sealantsand adhesives provide the insulating glass assembly with sufficientstrength. In high-quality insulating glass systems designed to meetmodern standards, a sealant acting as a barrier against water vapor isarranged between those surfaces of the spacer which face the glasspanels and the surface of the glass. Thermoplastic formulations based onpolyisobutylene and/or butyl rubber are generally used for this purpose.The production of such insulating glass assemblies generally involves anumber of complex steps and is still very expensive despite the highdegree of automation found in large production lines. Accordingly,numerous attempts have been made to simplify the complex steps involvedin the production of insulating glass and, in particular, to eliminatethe need for pre-profiled spacers.

[0004] In the so-called Biver system, for example, a thermoplasticstrand, which is preferably based on polyisobutylene or butyl rubber andwhich may contain a molecular sieve to absorb moisture, is firstextruded onto one panel around its edges. The second panel is thenpositioned over the first, after which the two panels are pressedtogether to the predetermined distance. The outer edge region is thensealed by a generally two-component adhesive/sealant. This system isdescribed in numerous patents/applications, for example in DE-C-2555381,DE-A-2555383, DE-A-2555384 and in EP-A-176388 or EP-A-714964.

[0005] In order to facilitate flexible coupling of the panels and toobtain a dimensionally stable, self-supporting assembly, WO 94/16187proposes the use of shaped bodies of a textile as the spacer between theglass panels. The textile spacer contains highly elastic but rigid linkfilaments and is impregnated with a resin as binder to form the edgeseal. To this end, the edge of one panel is covered with theresin-impregnated textile spacer. The second panel is then placedexactly over the first, after which the two panels are pressed togetherto join them at their edges. After the press has been opened, thereactive binder system is left to cure.

[0006] WO 97/31769 describes a preformed flexible laminate for formingthe edge seal between insulating glass panels. This flexible laminatecontains a wavy flat material partly or completely embedded in its corematerial as spacer, its surface extending perpendicularly of the glasspanels. On at least one surface, the laminate has a polymeric coatingwhich seals off the interior of the panel assembly against air and/ormoisture and maintains the required distance between the glass panels.Laminates of the type in question are produced by a multi-stepco-extrusion process in which the wavy flat material is first embeddedin a core material which then has to be coated with one or morepolymeric materials on its outer surfaces.

[0007] According to EP-A-81656, two-panel insulating glass is producedby first coating the edges of the glass panels to be joined with asolution of a primer or adhesive. The glass panels are then brought tothe predetermined distance apart and a thermoplastic resin compositionof a butyl rubber and a crystalline polyolefin, which may also containtackifiers and drying agents, is extruded into the edge region.

[0008] The disadvantage of all the above-mentioned edge sealing systemsbased on thermoplastic polymers lies in their poor heat resistance andlong-term temperature resistance. These disadvantages can only beovercome by using reactive systems of the reactive hotmelt adhesive typewhich post-crosslink either thermally or under the effect of moisture oroxygen so that a crosslinked polymer matrix around the edge of theinsulating glass system provides for adequate thermal stability. Thus,WO 97/15619 describes sealants/adhesives for the production ofinsulating glass units based on one-component, hot-applied, chemicallycrosslinking adhesives/sealants. These binder systems contain athermoplastic hotmelt adhesive resin mixed with a resin which can becrosslinked with atmospheric oxygen and/or moisture. The hotmeltadhesive resin acts as a fusible component during the originalapplication and establishes early strength immediately after cooling.The crosslinkable polymer phase then begins to react by crosslinkingwith the oxygen or moisture in the surrounding air. The crosslinkableresins mentioned include moisture-reactive polyurethanes,moisture-reactive polysulfides, polydimethyl siloxanes or oxygen-curingpolysulfides.

[0009] DE-A-19821356 describes a process for the production of asilane-modified butyl rubber in which a butyl rubber is reacted with amercaptofunctional silane containing hydroxy groups or hydrolyzablegroups in the presence of a radical former. According to the teaching ofthis document, such polymers can be mixed with other additives in akneader, processed to form a two-component composition and applied toglass by means of a suitable machine. The applied composition then actssimultaneously as a spacer for the two glass panels, contains a dryingagent for the inter-panel gap and acts as a water vapor and gas barrierand as an elastic bond.

[0010] WO 97/48778 describes a hotmelt adhesive composition containing amixture of at least one reactive binder based on silane-functionalpolyisobutylenes, hydrogenated polybutadiene and/or poly-α-olefins and anon-reactive binder from the group of butyl rubbers, poly-α-olefins,polybutenes, styrene block copolymers or diene polymers. These hotmeltadhesive compositions may be used as one- or two-componentadhesives/sealants for the production of insulating glass. There is noneed for separate spacers of metal or plastic profiles.

[0011] Besides some processing-related advantages, the various systemsdescribed in the foregoing have certain disadvantages. The Biver systemrequires a thermoplastic spacer (TPS) and a conventional, generallytwo-component adhesive based on polysulfide, silicone or polyurethane.Although, in the case of reactive hotmelt adhesives, only one materialis generally required, both the above-mentioned binder systems aresupplied in drums from which the material is pumped to the point ofapplication, optionally after heating. Problems can arise duringprocessing if, in cases where the volume of material called up per unitof time is high, the quantity melted in the reservoir of the applicatorand the melting rate per unit of time are not sufficient to guaranteethe necessary flow of material. In addition, the reactive one-componentwarm- or hot-melting systems are attended by the problems familiar tothe expert, such as difficulties during packaging, poor stability instorage and a low curing rate and during the disposal/cleaning of theused adhesive-contaminated containers.

[0012] Against the background of this prior art, the problem addressedby the present invention was to provide a binder system which would lenditself to application in the same way as reactive hotmelt adhesives, butwhich would provide for improved storage, feeding and transportation inrelation to the prior art. In particular, the binder system would beeasy to handle and to dose, even after prolonged storage at varioustemperatures. This would also include avoiding contamination of thetransit containers. In addition, the reactive components would lendthemselves to rapid melting and mixing. Neither the adhesive propertiesnor the water vapor and gas barrier effect would be adversely affected.

[0013] The solution to the problem stated above is defined in the claimsand consists essentially in the provision of a reactive blend ofthermoplastic polymer particles based on poly-α-olefins, elastomericblock copolymers and/or polyisobutylenes,

[0014] a) a proportion of the blend particles containing polymers withreactive groups selected from hydroxyl groups, amino groups, carboxylgroups, carboxylic anhydride groups, mercapto groups, silane groupsand/or hydrosilyl groups and

[0015] b) another proportion of the blend particles containing polymerswith reactive groups selected from isocyanate groups, epoxide groups,active olefinically unsaturated double bonds and/or water-containing orforming substances and

[0016] c) optionally a further proportion of the blend particlescontaining auxiliaries and additives which do not react with thefunctional groups of the a) and b) particles.

[0017] The elastomeric block copolymers according to the inventioninclude in particular the di- and tri-block copolymers of styrene withbutadiene or isoprene and hydrogenation products thereof, for examplestyrene/butadiene/styrene (SBS), styrene/isoprene/styrene (SIS),styrene/ethylene/butylene/styrene (EBS) andstyrene/ethylene/propylene/styrene (SEPS).

[0018] The present invention also relates to a process for joining flatmaterials, more particularly insulating glass panels, which essentiallycomprises the following steps:

[0019] a) homogenizing and melting the above-mentioned reactive blend,optionally in an inert atmosphere with no moisture and/or oxygen, usinga high-shear, optionally heatable mixing unit,

[0020] b) extruding the homogenized reactive thermoplastic mixture,optionally through a shaping nozzle, onto at least one edge of a flatmaterial,

[0021] c) subsequently fitting a second matching flat material onto theapplied layer of the reactive mixture,

[0022] d) optionally mechanically fixing and/or pressing the fitted flatmaterial,

[0023] e) cooling the composite system of flat materials thus formed toroom temperature, the reactive mixture curing by crosslinking.

[0024] The present invention also relates to the production of two-panelor multi-panel insulating glass, sheet-form casting resins, solarcollectors or facade elements for buildings by the process describedabove.

[0025] Blend particles in the context of the present invention areunderstood to be polymer-containing mixtures which largely retain theirshape at room temperature. Room temperature in the present context is atypical storage temperature between 0° C. and about 30° C. The particlesare granules with mean diameters between 0.5 and 40 mm, preferablybetween 1 and 30 mm and more particularly between 2 and 20 mm. Inprinciple, the particles may have any shape, their shape largely beingdetermined by the process used for their production. In one particularlypreferred embodiment, the granules are produced by extrusion through amultiple-bore die and the strands thus extruded are cut to the requiredlength. The granules may be both spherical and disk-like, cube-like,elliptical or cylindrical in shape.

[0026] Besides the reactive components a) and b), the granules alsocontain polyisobutylene, poly-α-olefins, elastomeric block copolymers,waxes and fillers, pigments, optionally water-binding agents in the formof molecular sieves (drying agents). The granules and particularlycomponent c) may also contain auxiliaries and additives, such ascatalysts, flow aids, antiagers and also drying agents, dyes andpigments.

[0027] By virtue of the presence of poly-α-olefins and particularlypolyisobutylene and partly by virtue of the presence of the reactiveconstituents, the granules have a tacky surface immediately they leavethe extruder or granulator so that they would agglomerate in the eventof prolonged storage. In general, therefore, the granules aresurface-coated with a suitable release agent immediately aftergranulation. The release agent may consist, for example, of a mixture oftalcum, pyrogenic silica and molecular sieve powder. However, otherpowder-form release agents may also be used for surface-coating,including for example carbon black, highly disperse silicas without theother constituents mentioned above, polyethylene powder, ethylene/vinylacetate powder or other fine-particle polymer powders. Release agentscapable of being melted at slightly elevated temperatures, such as waxesfor example, may also be sprayed onto the surface of the granules.Examples of such waxes are polyolefin waxes, particularly polyethylenewax, and even Fischer-Tropsch wax. The key selection criterion is thatthe particle surface should not be tacky at room temperature and storagetemperature. However, the layer of release agent should lend itself toincorporation in the binder system without any incompatibility duringfurther processing by the end user. This outer non-tacky layer shouldsurround the core of the granule so completely that the surface layercan be said to be continuous, i.e. generally more than 90% and inparticular more than 99% of the granule surface is coated. The granulesthus flow freely. In other words, the granules flow freely through anopening under their own weight, even after prolonged storage attemperatures of up to 30 or 40° C., and can therefore be transportedwithout difficulty.

[0028] Typically, the non-reactive constituents of the blend particlesare present in the following quantities:

[0029] poly-α-olefins and/or elastomeric block copolymers: 5 to 30% byweight,

[0030] polyisobutylene: 20 to 50% by weight,

[0031] wax: 0 to 10% by weight, preferably 0.5 to 5% by weight

[0032] fillers: 10 to 30% by weight,

[0033] carbon black: 5 to 30% by weight, preferably 5 to 20% by weight,

[0034] molecular sieve: 10 to 20% by weight,

[0035] optionally catalysts, flow aids, antiagers: 0.5 to 8% by weight,

[0036] reactive polymer: 2 to 30% by weight, preferably 5 to 20% byweight.

[0037] Accordingly, the non-reactive binders are essentially formed fromthe group of poly-α-olefins, rubbers based on styrene block copolymerswith dienes such as, for example butadiene or isoprene, these blockcopolymers optionally being completely or partly hydrogenated. Rubbersbased on statistical diene homo- and/or copolymers may also be used.Another key constituent are butyl rubbers in the form of polybutenes orpolyisobutylenes. Examples of poly-α-olefins are ethylene/propyleneelastomers, such as ethylene/propylene copolymers for example, andterpolymers of ethylene and propylene with an unconjugated diene (EPDM)or propene/butene copolymers and ethylene/vinyl acetate.

[0038] The rubbers based on styrene block copolymers are mainly di- andtri-block copolymers of styrene with a diene such as, for example,butadiene or isoprene which are commercially available, for example,from Shell under the name of “Kraton”. As already mentioned, these blockcopolymers may also be used in their hydrogenated or partly hydrogenatedform.

[0039] Examples of the statistical diene homo- and copolymers arepolybutadiene, polyisoprene, copolymers thereof and statisticalstyrene/butadiene copolymers (SBR), acrylonitrile/butadiene copolymers(NBR) and the partly hydrogenated or completely hydrogenated dienepolymers of the last-mentioned group.

[0040] By virtue of their well-known and particularly good water vaporor gas barrier effect, the polybutenes and/or polyisobutene, i.e. thepolyolefins produced by stereospecific polymerization of 1-butene orisobutene, and the butyl rubbers, i.e. copolymers of isobutylene withisoprene, are a particularly preferred key constituent of the granules.

[0041] The reactive thermoplastic polymer granules according to theinvention additionally contain constituents known per se, including inparticular water-binding fillers, preferably zeolites of the 3A typeknown as molecular sieves or powder-form calcium oxide. Fine-particleinert fillers, for example ground or precipitated chalks, kaolins, claysand carbon blacks, may also be used. The chalks, kaolins or clays may beused both in their surface-hydrophobicized form and without any surfacepretreatment.

[0042] In addition, at least some of the thermoplastic polymer granulesmay contain organofunctional silanes as coupling agents and/orcrosslinking agents, including for example 3-glycidyloxypropyltrialkoxysilane, 3-acryloxypropyl trialkoxysilane, 3-aminopropyltrialkoxysilane, vinyl trialkoxy silane, N-aminoethyl-3-aminopropyldialkoxysilane, vinyl aminopropyl trialkoxysilane or aminoalkyltrialkoxysilane. Particularly preferred alkoxy groups are methoxy andethoxy groups.

[0043] The choice of the antiager optionally used is determined by thecomposition of the binder. Antioxidants of the sterically hinderedphenol, thioether or high molecular weight mercapto compound type, UVfilters of the known benzotriazole, benzophenone or HALS (hindered aminelight stabilizer) type may be used as antiagers. It can be useful to addknown antiozonants and, in exceptional cases, hydrolysis stabilizers mayalso have to be added.

[0044] The reactive constituents of the thermoplastic granules arepolymers or oligomers containing reactive groups. The polymers of groupsa) and b) may be selected from polymers containing on average more thanone functional group, preferably 2 to 2.5 groups. These reactive groupsfor the polymers of group a) may be selected from hydroxyl groups, aminogroups, carboxyl groups, carboxylic anhydride groups, mercapto groups,silane groups and/or hydrosilyl groups.

[0045] The reactive groups of the group b) polymers should of course becomplementary to the group a) polymers so that a two-component reactivesystem is latently present here. The reactive groups of the group b)polymers may be selected from isocyanate groups, epoxide groups, activeolefinically unsaturated double bonds and/or water-binding substances orsubstances which contain adsorbed water and are capable of releasing it.

[0046] Actual examples of the group a) polymers are polybutadienes andpolyisoprenes containing predominantly terminal OH groups, amino groups,carboxyl groups, carboxylic anhydride groups or mercapto groups whichmay optionally be completely partly hydrogenated. Polybutadienescontaining alkoxysilane groups may also be used. The silane-functionalpolyisobutylenes, silane-functional hydrogenated polybutadienes and/orsilane-functional poly-α-olefins described on pages 5 to 6 of WO97/48778 may also be used.

[0047] The reactive polymer and/or oligomer used for component b) may bean isocyanate-terminated polybutadiene obtainable, for example, by thereaction of OH-functional polybutadiene with a diisocyanate such as, forexample, diphenylmethane diisocyanate (MDI), toluene diisocyanate (TDI)or similar di- and polyisocyanates well-known from polyurethanechemistry. In the most simple case, component b) may even be the homologmixture of multinuclear MDI homologs of the so-called “crude MDI” type.A component b) containing isocyanate groups is of course preferablycombined with a hydroxyfunctional or aminofunctional or evenmercaptofunctional component a).

[0048] In the most simple case, the epoxyfunctional component b) isselected from glycidyl ethers of polyphenols, i.e. glycidyl ethers ofbisphenol A or the novolaks. However, relatively high molecular weightepoxy resins obtainable by reaction of diglycidyl ethers of bisphenol Awith, for example, isocyanate prepolymers may also be used. Anepoxyfunctional component b) is preferably combined with anaminofunctional, carboxyfunctional, carboxylic anhydride-functional ormercaptofunctional component a). If component b) contains activeolefinically unsaturated double bonds as reactive groups in the polymer,it should be combined with a polymer component a) containing hydrosilylgroups. Another possibility is to combine highly reactive acrylate ormethacrylate polymers of group b) with mercaptofunctional polymers ofgroup a) (so-called “thiol-ene” reaction). However, the (meth)acrylatepolymers of group b) may also be combined with aminofunctional polymerparticles a) which then enter into a Michael addition reaction duringcrosslinking.

[0049] The catalysts to be used in the thermoplastic reactive granulesare determined by the reactive system selected and are known inprinciple to the expert. Examples of suitable catalysts are polyurethanecatalysts from the group of organometallic compounds of tin, iron,titanium, bismuth, aliphatic tertiary amines and, in particular, cyclicaliphatic amines. Examples of epoxy catalysts are tertiary amines, Lewisacids or salts thereof or complex compounds thereof with organic amines.Catalytically active tertiary alkylamines such as, for example,tris-(dimethylamino)-phenol, piperidine, piperidine derivatives orimidazole derivatives may also be used as catalyst for the epoxides.Suitable crosslinking catalysts for silane-functional polymers are theorganometallic compounds, tertiary amines or acids also used inpolyurethane chemistry. The catalysts may be added either to thenon-reactive component c) or to one of components a) or b). For example,the polyurethane catalysts may be added to component a) which containshydroxyfunctional, aminofunctional or mercaptofunctional polymers.

[0050] The individual components a), b) and/or c) are first prepared byhomogenizing the mixture components in a kneader, internal mixer orsimilar mixing unit, extruding the resulting mixture through a suitableextrusion die—for example a multiple bore die—and then size-reducing theextruded strands into granules. After the granules have beensurface-coated with the above-mentioned release agents, the individualcomponents a), b) and c) are packed in the necessary quantity ratios inthe storage or transit container. It may be necessary, for example inthe case of isocyanate-functional components or silane-functionalcomponents, to seal the container against moisture after it has beenfilled. The container may be selected from a broad range of containersincluding, for example, the conventional 200 liter drums, large-volumepouring containers or large-volume flexible containers of the so-called“big bag” type. The only condition that suitable storage or transitcontainers have to satisfy is that they should if necessary be sealableagainst moisture and should enable the flowable granules to be removedeither by gravity or, for example, by pneumatic feed systems.

[0051] At the end user, the granules according to the invention mayreadily be removed from the storage container because they flow freelyor are flowable and can then easily be fed to the mixing unit. There areno dosing problems because the reactive particles a) and b) have alreadybeen mixed in the correct ratio by the manufacturer. The mixing unitmust be of a high-shear type because the granules are shattered in themixing unit, optionally after heating, and form a homogeneous mass sothat the two reactive components a) and b) are mixed together. Afterthis homogenization, the thermoplastic melt is applied, optionallythrough a shaping nozzle, to at least one edge of a flat material, forexample a panel of glass. The second flat material is then positionedexactly onto the surface of the extruded reactive thermoplasticmaterial. The two flat materials are then optionally pressed and left tocool, the edge bond immediately having sufficient early strength forfurther processing.

[0052] The mixture may be heated either by external heating units or bythe energy of the high-shear mixing process.

[0053] Actual examples of suitable high-shear mixing units aresingle-screw and multiple-screw extruders, kneaders with a dischargescrew optionally preceded by a static mixer, (co)kneaders,multiple-chamber mixers or mixing units of the type used for theproduction of bulk molding compounds or special dough molding compoundsand co-called Konterna mixing units (manufacturer Ika).

[0054] In principle, however, the particle mixtures according to theinvention may also be applied from small applicators, for example fromconventional cartridges. To this end, the cartridges optionally have tobe heated and the piston moved by compressed air, hydraulically ormechanically in order to force the molten granules out of the cartridgeopening. The cartridge may be preceded by a static mixer known per se asthe high-shear mixer. Static/dynamic mixing systems as disclosed, forexample, in WO 95/24556 may also be used. Static/dynamic mixing systemsas disclosed in EP-A-313519, EP-A-351358 and in DE-U-8717424 are alsosuitable.

[0055] The reactive blends of thermoplastic polymer particles accordingto the invention are preferably used for the production of insulatingglass, They may also be used for the production of solar collectors orsolar elements and for the production of facade elements of glass orsheet-like materials similar to glass which have to beflexibly/elastically joined at their edges. The compositions accordingto the invention may also be used for the production of sheet-formcasting resins and for the edge sealing of safety glass.

[0056] The following Examples are intended to illustrate the inventionwithout limiting it in any way. Unless otherwise indicated, allquantities in the following Examples are percentages or parts by weight,based on the composition as a whole.

EXAMPLES

[0057] In the following Examples, the formulation ingredients were mixedin vacuo to homogeneity in the absence of air in a laboratory kneader.

[0058] In order to test stability in storage, some of the resultingmixture was introduced into moisture-proof cans which were then closed.The material retained its reactivity and crosslinkability after storagefor several weeks in the closed container.

[0059] In order to test the curing properties, another part of themixture was pressed to 50 mm diameter and 10 mm thick disks and theprogress of curing was measured by penetration measurement by the conepenetration method to ASTM D 217. The cone angle was 30°, the weight 150grams and the penetration time 6 seconds. Penetration was measured onthe one hand immediately and on the other hand after storage for severaldays in a standard conditioning atmosphere (DIN 50014). The firstmeasurement was intended to determine the progress of curing in ambientconditions, the second was intended to determine accelerated curing.

[0060] In order to determine tensile strength, another part of thematerial was pressed to 13-14 mm thick plates and cut into 1 cm wide and5 cm long strips. The strips were placed centrally on a 5 cm×5 cm plateof glass, after which a second glass plate was positioned on theadhesive/sealant strips so that the two glass plates were congruent.With the assistance of spacers, the two glass plates were pressed to adistance of 12.5 mm so that the adhesive/sealant strip completely wettedboth glass plates and had dimensions of 12.5×10×50 mm. Tensile strengthwas then determined in an Instron laboratory tensile tester after thetest specimens had been stored for 1 day at 80° C. and for several daysat 80° C. TABLE Example 1 2 3 4 5 6 Polyisobutylene¹ 145 145 145 145 145167 Polyethylene wax² 5 5 5 5 5 5.8 Chalk³ 90 90 90 90 90 103.7 Carbonblack⁴ 100 100 100 100 100 115.2 Polybutene/isobutene⁵ 10 10 10 10 1011.5 Molecular sieve 3A (powder) 65 65 65 65 65 74.9 SEBS polymer⁶ 100100 100 EB polymer⁷ 20 Maleinized polybutadiene⁸ 137.4 68.7OH-functional 56 28 polybutadiene⁹ NCO-functional 100 100 115.2polybutadiene¹⁰ Silane-functional 100 polyisobuylene¹¹ Polyetherplasticizer 6 Glymo¹² 5 5 5 5.76 Potassium octoate 2 DBTL¹³ 1 1 1.15Dibutyl tin acetyl acetonate 1.5 Penetration¹⁴ (immediate) 93 34 12 1926 Penetration (x days NK)¹⁵ 34d-10 63d-20 14d-5 15d-12 12d-17Penetration (x days 80° C.) 34d-1  63d-8  14d-2 15d-5  12d-6  Shore A(final value after 80 77 curing) Tensile strength (1 day 0.5 0.5 0.7 1.280° C.) [Mpa] Tensile strength (x days 50d/0.8 15d/1.5 14d/1.5 14d/1.480° C.) [Mpa]

[0061] The molecular sieve used had a water content of ca, 3%.

Example 7

[0062] Blend particles for component a) and component b) were separatelyproduced in a kneader in accordance with Examples 1 to 6. Component a)Polyisobutylene¹ 145 parts OH-functional polybutadiene² 100 parts Chalk³ 90 parts Carbon black (Printex, U)⁴ 100 parts Molecular sieve 3A(powder)  65 parts DBTL⁵  2 parts Component b) Polyisobutylene¹ 145parts NCO-terminated polybutadiene² 100 parts Chalk³  90 parts Carbonblack (Printex, U)⁴ 100 parts Molecular sieve 3A (powder)  65 partsExample 8 Component a) Polyisobutylene¹ 145 parts OH-functionalpolybutadiene²  56 parts Chalk³  90 parts Carbon black (Printex, U)⁴ 100parts Molecular sieve 3A (powder)  65 parts Component b)Polyisobutylene¹ 145 parts Maleinized polybutadiene² 137 parts Chalk³ 90 parts Carbon black (Printex, U)⁴ 100 parts Molecular sieve 3A(powder)  65 parts

[0063] Granules were produced from components a) and b) produced inExamples 7 and 8 by extruding 8 mm diameter strands of material andcutting the strands into 8 mm long pieces. The granules were packedimmediately afterwards in moisture-proof cans. The granules still hadtheir original reactivity after storage for several weeks.

[0064] For further processing, equal parts of components a) and b) arehomogenized and extruded into the corresponding mold. After the materialhas cured completely, its physical and mechanical data can bedetermined. The strength values obtained are largely consistent withthose obtained in Examples 1 to 6.

1. A reactive blend of thermoplastic polymer particles based on butylrubber, elastomeric block copolymers, poly-α-olefins and/orpolyisobutylenes, characterized in that a) a proportion of the blendparticles contains polymers with reactive groups selected from hydroxylgroups, amino groups, carboxyl groups, carboxylic anhydride groups,mercapto groups, silane groups and/or hydrosilyl groups, b) anotherproportion of the blend particles contains polymers with reactive groupsselected from isocyanate groups, epoxide groups, active olefinicallyunsaturated double bonds and/or water-forming or containing substancesand c) optionally a further proportion of the blend particles containsauxiliaries and additives which do not react with the functionalpolymers of the a) and b) particles.
 2. A reactive blend as claimed inclaim 1, characterized in that the reactive constituents of parts a) andb) of the blends are present in substantially stoichiometric quantities.3. A reactive blend as claimed in claim 1 or 2, characterized in thatthe auxiliaries and additives are selected from catalysts, dryingagents, flow aids, antiagers and/or dyes and pigments.
 4. A reactiveblend as claimed in at least one of the preceding claims, characterizedin that the particles of parts a), b) and optionally c) of the blend aregranules with mean particles sizes of 0.5 to 40 mm, preferably 1 to 30mm and more particularly 2 to 20 mm.
 5. A reactive blend as claimed inclaim 4, characterized in that the surface of the granules is treatedwith tack-reducing and/or moisture-binding agents.
 6. A reactive blendas claimed in claim 5, characterized in that the tack-reducing agentsare selected from fine-particle powders in the form of carbon black,highly disperse silica, polyethylene powder or talcum or fromlow-melting liquids which can be sprayed on or—in solid form—dusted on,such as waxes or paraffins.
 7. A process for joining flat materials,characterized by the following key steps: a) homogenizing and meltingthe above-mentioned reactive blend claimed in at least one of claims 1to 6, optionally in an inert atmosphere with no moisture and/or oxygen,using a high-shear, optionally heatable mixing unit, b) extruding thehomogenized reactive thermoplastic mixture, optionally through a shapingnozzle, onto at least one edge of a flat material, c) subsequentlyfitting a second matching flat material onto the applied layer of thereactive mixture, d) optionally mechanically fixing and/or pressing thefitted flat material, e) cooling the composite system of flat materialsthus formed to room temperature, the reactive mixture curing bycrosslinking.
 8. Production of two-panel or multi-panel insulatingglass, sheet-form casting resins, solar collectors, fagade elements forbuildings by the process claimed in claim 7.